Marking having electroluminescent lighting effect, method for  the production thereof

ABSTRACT

An electroluminescent arrangement is described. This electroluminescent arrangement comprises the following functional layers:
         (a) rear electrode as layer A;   (b) dielectric layer as layer B;   (c) electroluminescent layer as layer C; and   (d) cover electrode as layer D.

The present invention relates to electroluminescent arrangements, aprocess for their production, as well as their use in particular asdistinguishing/identification signs for vehicles. The invention alsoprovides a front diaphragm blank as well as a process for itsproduction.

Electroluminescence (hereinafter also abbreviated to “EL”) is understoodto mean the direct excitation of luminescence from luminescent pigmentsor luminophores by an alternating electric field.

Electroluminescence technology has recently become increasinglyimportant. This technology enables homogeneous luminous surfaces free ofdazzle and shadow and of virtually any desired size to be formed. At thesame time the power consumption and structural thickness (of the orderof magnitude of a millimetre or less) are extremely low. Typical usesinclude, apart from the background illumination of liquid crystaldisplays, the back-lighting of transparent films that are provided withlettering and/or image motifs. Thus, transparent electroluminescentarrangements, for example electroluminescent luminous boards based onglass or transparent plastics, which can serve for example asinformation carriers, advertising panels, or for decorative purposes,are known from the prior art.

A zinc sulfide electroluminescent arrangement based on the use of twoelectrodes of conducting glass with an electroluminescent phosphorarranged therebetween was already described in 1950 by E. C. Payne inU.S. Pat. No. 2,838,715, and a publication by G. Destriau “The NewPhenomenon of Electroluminescence and its Possibilities for theInvestigation of Crystal Lattice” in the “Philosophical Magazine” wasmentioned by way of reference, in which connection the originaldiscovery of the particular ZnS EL phenomenon in an alternating voltagefield was already made by Destriau in 1936.

The luminescent pigments and luminophores that are used in these ELelements are embedded in a transparent, organic or ceramic binder. Thestarting substances are generally zinc sulfides, which depending ondoping or co-doping and preparation procedure generate different,relatively narrow-band emission spectra. The reason for the use of zincsulfides in the EL layers is due on the one hand to the relatively largenumber of zinc sulfide EL pigments that are available. The centre ofgravity of the spectrum at the same time determines the respectivecolour of the emitted light. The emission colour of an EL element can bematched by means of a large number of possible measures to the desiredcolour impression. These measures includes the doping and co-doping ofthe luminescent pigments, the mixing of two or more EL pigments, theaddition of one or more organic and/or inorganic colour-convertingand/or colour-filtering pigments, the coating of the EL pigment withorganic and/or inorganic colour-converting and/or colour-filteringsubstances, the admixture of colorants to the polymer matrix in whichthe luminescent pigments are dispersed, as well as the incorporation ofa colour-converting and/or colour-filtering layer or film in thestructure of the EL element. In general, depending on the employeddoping and co-doping of the zinc sulfide pigments a relativelybroad-band emission spectrum is produced if a suitably high alternatingvoltage of normally greater than 50 volts up to more than 200 volts anda frequency of greater than 50 Hz up to a few kHz, normally in the rangefrom 400 Hz to 2 kHz, is applied.

In order that the produced emission can be seen, at least one flat(planar) electrode is preferably designed to be largely transparent.

Depending on the intended use and production technology, glasssubstrates or polymeric films with an electrically conducting andlargely transparent coating can be used for this purpose. In specialembodiments an EL capacitor structure can also be arranged on asubstrate in such a way that as front transparent electrode only a thinlayer is printed or knife coated, or applied by a roller coating method,a curtain casting method or a spray method. In principle both flatelectrodes can also be made largely transparent and in this way atranslucent EL element is formed that exhibits a light emission on bothsides.

Electroluminescent arrangements are used for example in the field ofself-luminescent number plates for vehicles.

Self-luminescent number plates (abbreviation “SLN”), also termed“self-luminescent distinguishing signs” or “self-luminescentdistinguishing plates”, are vehicle distinguishing signs that do nothave to be illuminated in the dark by an external light source in orderthat they can be read, but emit light themselves.

At the present time there exist two different types of self-luminescentnumber plates which are commercially available:

-   -   In one type of self-luminescent number plates the lettering is        produced by embossing a translucent, white reflecting plastics        plate, behind which are arranged white LEDs. For this system,        which was developed by the 3M® company, a general model and        design approval (ABG) was granted by the German Federal Highways        Authority on 10 Jul. 2006.    -   In a second type of self-luminescent number plates the lettering        is printed on a transparent film, which in turn is bonded to an        electroluminescent film. The electroluminescent film lights up        when an electrical voltage is applied to the film. Number plates        according to this principle have likewise been authorised by the        German Federal Highways Authority (ABG K55 of 27 Feb. 2007).

Corresponding electroluminescent systems are also known from theprinting technology prior art.

For example, from WO 03/064210 A1 a plate, in particular anidentification or number plate for vehicles, with a base body is known,wherein the base body consists of an electrically conducting material orcomprises an electrically conducting coating to form a first electrodedirectly or via a further layer. A coating containing electroluminescentpigmentation is applied to the base body or to the electricallyconducting coating, which pigmented coating is in turn covered with anelectrically conducting transparent layer to form a second electrode.The base body or the base body with the electroluminescent layer and theelectrically conducting transparent layer for forming the secondelectrode can be shaped, and in particular can be embossed.

In EP 1 463 654 A1 a plate, in particular a vehicle identificationplate, is described, which comprises a support made of a plasticallydeformable material, for example of metal, and an electroluminescentlayer structure so as to form at least one flat capacitor. Theelectroluminescent layer structure has a base electrode, an insulatinglayer, a pigment layer that luminesces in operation, and a transparentcover electrode. A further insulating layer is applied to the support,above which insulating layer is arranged an electrically conductinglayer from which are fashioned the base electrode and at least one powersupply lead, electrically separate therefrom, for the cover electrode ofthe at least one flat capacitor. The further insulating layer is aplastics film that is first of all continuously coated with anelectrically conducting material on the side facing away from thesupport, the said insulating layer having a bracket projecting beyondthe support and on which are formed the connection leads necessary forthe contacting of the base electrode and the power supply lead.

In EP 0 978 220 A a plastics moulded article with an EL thick-filmelement is described, wherein this EL thick-film element isthree-dimensionally shaped and sprayed on the back with thermoplasticmaterial at an operating temperature below the softening point of thefilm, and in this way a three-dimensional self-luminescent mouldedarticle is produced.

In German Patent Application DE 10 2006 031 315 of earlier priority datebut not prior-published, entitled “3D-EL-HDVF element and productionprocess and use”, a process is described for the production of athree-dimensionally shaped and graphically configured plastics filmelement consisting of at least one graphically configured plastics filmcold-stretchable below the softening point and at least one protectivefilm element, wherein the originally flat and cold-stretchable film withthe various cold-stretchable graphical printing together with at leastone protective film is moved in an isostatic high-pressure shaping tool,and at a process temperature below the softening point of the plasticsfilm is three-dimensionally shaped in a stress-whitening-free mannerwith a fluid compression agent at a pressure greater than 20 bar, is atthe same time laminated, and is then cut along the edges. In additionthe graphical printing is provided with functional properties like aninorganic printable electroluminescent layer sequence.

These distinguishing signs with an electroluminescent effect known fromthe prior art still have disadvantages in many respects.

Thus, the distinguishing signs with an electroluminescent effect knownfrom the prior art all have the disadvantage that a simple, secure andeasily applicable contacting of the distinguishing sign with for examplethe electrical circuit of the vehicle is not possible. For example, thecontacting device described in the aforementioned EP 1 463 654 A anddesigned as a bracket is complicated to produce. In addition thisbracket interferes in the further processing, in particular in thelamination. The cost-effective roll-to-roll lamination process isdifficult to execute in this form of implementation, since in thisprocess the bracket is located in the contact region between two endlesssupports and would have to be machined out in a complicated procedureonly later. Furthermore the exposure of the bracket necessitates theprovision of diffusion barriers against moisture, since the luminophoresare sensitive to moisture and the conducting parts suffer fromelectrical corrosion under the action of moisture.

Moreover, corresponding distinguishing signs with an electroluminescenteffect are often also shaped three-dimensionally, such as for example inthe embossing of a distinguishing sign for a vehicle. As a result theelectrically conducting coatings can fracture and break, especially inthe electrodes. These fractures can mean that electrical conductivity isnot ensured over the whole electrode.

Quite apart from this, the cold working property (formability) ofcorresponding electroluminescent elements is generally not alwayssatisfactorily achieved.

With the automobile distinguishing signs having an electroluminescenteffect known from the prior art, in addition the bonding to thesubstrates is not satisfactorily achieved. Thus, correspondingtransitions between the electroluminescent arrangement and substrate inthe systems known from the prior art are neither sufficiently stable norsufficiently durable. Moreover, the transitions do not exhibit adequateshaping properties, which is essential of course especially whenembossing automobile distinguishing signs with electroluminescenteffects. For example, when embossing an automobile distinguishing signan embossing of two angles of 90° at a height of 2 mm is generallynecessary. In addition the reflecting properties of the automobiledistinguishing signs with an electroluminescent property known from theprior art also need to be improved.

Accordingly, the present invention is involved with the object ofimproving electroluminescent arrangements of the aforementioned type invarious respects, especially in the areas identified above as critical.

This object is achieved by the electroluminescent arrangement accordingto the invention.

The electroluminescent arrangement according to the invention ischaracterised in that the arrangement comprises the following functionallayers:

(a) Rear electrode as component BE;(b) dielectric layer as component BD;(c) electroluminescent layer as component BC; and(d) cover electrode (=front electrode) as component BA.

The electroluminescent arrangement according to the invention is basedin general on an inorganic thick-film AC system, which can be producedfor example using conventional flat bed and/or cylinder silk-screenprinting machines. The production of the electroluminescent arrangementaccording to the invention is thus possible in a simple manner usingconventional and available equipment.

The structural arrangement of the electroluminescent element accordingto the invention is described in more detail hereinafter.

The electroluminescent element according to the invention comprises atleast one EL layer as layer BC. The layer BC can also be formed fromseveral layers having an electroluminescent effect. The at least oneelectroluminescent layer (component BC) is generally arranged betweenthe cover electrode (component BA) and the dielectric layer (componentBD). In this connection the electroluminescent layer can be arrangedimmediately adjacent to the dielectric layer (component BD) oroptionally one or more further layers can be arranged between thedielectric layer (component BD) and the electroluminescent layer(component BC). Preferably the electroluminescent layer (component BC)is arranged immediately adjacent to the dielectric layer (component BD).

In a further embodiment of the present invention the at least oneelectroluminescent layer (component BC) is generally arranged betweenthe rear electrode (component BA) and the dielectric layer (componentBD). In this connection the electroluminescent layer can be arrangedimmediately adjacent to the dielectric layer (component BD) oroptionally one or more further layers can be arranged between thedielectric layer (component BD) and the electroluminescent layer(component BC). Preferably the electroluminescent layer (component BC)is arranged directly adjacent to the dielectric layer (component BD).

Moreover, in the electroluminescent arrangement according to theinvention it is possible for the electroluminescent layer to consist oftwo or more electroluminescent layer elements arranged next to oneanother and having different electroluminescent phosphor pigments, sothat it is possible to produce different colours on theelectroluminescent arrangement.

In a further configuration the partial regions of the electroluminescentsurfaces can optionally be formed differently, for example as regardstheir composition, and can optionally be operated separately from oneanother. In this way different emission colours can be generated.

Structure of Electroluminescent Arrangements According to the Invention:

In a first particularly preferred embodiment of the present inventionthe electroluminescent arrangement consists of the following layers(normal structure):

-   a) an at least partially transparent substrate, component A,-   b) at least one electroluminescent arrangement, component B, applied    to the substrate and containing the following components    -   ba) an at least partially transparent electrode, component BA,        as front electrode,    -   bb) optionally an insulating layer, component BB,    -   bc) a layer containing at least one luminous pigment        (electroluminophore, El Phosphor) excitable by an electrical        field, termed an electroluminescent layer or pigment layer,        component BC,    -   bd) optionally an insulating layer, component BD,    -   be) a rear electrode, component BE, which can be at least        partially transparent,    -   bf) a conducting track or a plurality of conducting tracks,        component BF, for the electrical contacting of both component BA        as well as component BE, wherein the conducting track or the        conducting tracks can be applied before, after or between the        electrodes BA and BE, the conducting track or the conducting        tracks preferably being applied in one work step. The conducting        track or conducting tracks can be applied in the form of a        silver bus, preferably produced from a silver paste,        -   a graphite layer can possibly also be applied before the            application of the silver bus-   c) a protective layer, component CA, or a film, component CB.

The insulating layers BB and BD can be non-transparent, opaque ortransparent, in which connection at least one of the layers must be atleast partially transparent if two insulating layers are present.

Also, one or more at least partially transparent graphically configuredlayers can be arranged externally on the substrate A and/or between thesubstrate A and the electroluminescent arrangement.

Also, UV-blocking substances can be applied to and/or incorporated inone arbitrary side or on both sides of the substrate as well as in thesubstrate itself. In this way the service life of the luminophores canbe significantly extended; in particular the bleaching out or fading oforganic conversion pigments can thereby be dramatically slowed down.

Apart from the aforementioned layers (components A, B and C) theelectroluminescent element according to the invention (conventionalstructure) can comprise one or more reflecting layers. The reflectinglayer or layers can in particular be arranged as follows:

-   -   externally on the component A,    -   between the component A and component BA,    -   between the component BA and component BB, or BC if there is no        component BB,    -   between the component BD and component BE,    -   between the component BE and component BF,    -   between the component BF and component CA or CB,    -   externally on the component CA or CB.

Preferably the reflecting layer, where present, is arranged between thecomponent BC and BD, or BE if there is no component BD.

The reflecting layer preferably includes glass spheres, in particularhollow glass spheres. The diameter of the glass spheres can vary withinwide ranges. For example, they can have a size d₅₀ of in general 5 μm to3 mm, preferably 10 to 200 μm, particularly preferably 20 to 100 μm. Thehollow glass spheres are preferably embedded in a binder. In additionthe reflecting layer can contain metal particles; in this embodiment thereflecting layer is preferably arranged externally on the component Aand/or between the component A and component BA.

In an alternative embodiment of the present invention theelectroluminescent element consists of the following layers (reverselayer structure):

-   -   a) an at least partially transparent substrate, component A,    -   b) at least one electroluminescent arrangement, component B,        applied to the substrate and containing the following components        -   be) a rear electrode, component BE, that can be at least            partially transparent,        -   bb) optionally an insulating layer, component BB,        -   bc) a layer containing at least one luminous pigment            (electroluminophore) that can be excited by an electrical            field, called the electroluminescent layer or pigment layer,            component BC,        -   bd) optionally an insulating layer, component BD,        -   ba) an at least partially transparent electrode, component            BA, as front electrode,        -   bf) a conducting track or plurality of conducting tracks,            component BF, for the electrical contacting of component BA            as well as of component BE, wherein the conducting track or            conducting tracks can be applied before, after or between            the electrodes BA and BE, wherein preferably the conducting            track or conducting tracks are applied in one work step. The            conducting track or conducting tracks can be applied in the            form of a silver bus, preferably produced from a silver            paste. A graphite layer can possibly also be applied before            the application of the silver bus,    -   c) an at least partially transparent protective layer, component        CA and/or a film, component CB.

Also, one or more at least partially transparent graphically configuredlayers can be arranged on the transparent protective layer C and/orbetween the transparent protective layer C and the EL arrangement. Inparticular, the graphically configured layers can take over the functionof the protective layer.

In addition to the aforementioned layers (components A, B and C) theelectroluminescent element according to the invention with a reverselayer structure can include one or more reflecting layers. Thereflecting layer or layers can in particular be arranged as follows:

-   -   externally on component A,    -   between component A and component BE,    -   between component BE and component BB,    -   between component BB and component BC,    -   between component BC and component BD,    -   between component BD and component BA,    -   between component BA and component BF,    -   between component BF and component CA or CB,    -   on component CA or CB.

Preferably the reflecting layer, where present, is arranged betweencomponent BC and component BB, or BE if component BB is not present.Also, the reflecting layer can contain metal particles; in thisembodiment the reflecting layer is preferably arranged externally on thecomponent A and/or between the component A and component BE.

For the person skilled in the art it is obvious that the particularembodiments and features mentioned for the conventional structure applyas appropriate, unless otherwise stated, to the reverse layer structureand to the double-sided structure.

The one or more insulating layer(s) BB and/or BD in both theconventional structure as well as in the reverse structure can inparticular be omitted if the component BC has a layer thickness thatprevents a short circuit between the two electrodes, i.e. components BAand BE.

The individual function layers of the EL arrangements according to theinvention are described in more detail hereinafter:

(1) Electroluminescent Layer

The EL element according to the invention includes at least one ELlayer, component BC. The at least one EL layer can be arranged on thewhole internal surface of the first partially transparent electrode oron one or more partial surfaces of the first at least partiallytransparent electrode. In the case where the EL layer is arranged onseveral partial surfaces, the partial surfaces generally have a mutualinterspacing of 0.5 to 10.0 mm, preferably 1 to 5 mm.

The EL layer is in general composed of a binder matrix with EL pigmentshomogeneously dispersed therein. The binder matrix is generally chosenso as to produce a good adhesive bonding to the electrode layer (or tothe dielectric layer optionally applied thereto). In a preferredconfiguration systems based on PVB (polyvinyl butyral) or PU(polyurethane) are in this connection used for the binder system. Inaddition to the EL pigments optionally further additives may also bepresent in the binder matrix, such as colour-converting organic and/orinorganic systems, colorant additives for a daytime and nighttime lighteffect and/or reflecting and/or light-absorbing effect pigments such asaluminium flakes, glass flakes or mica platelets.

Preferably the at least one EL layer BC is an alternating currentthick-film powder electroluminescent (AC-P-EL) luminous structure.

In general the proportion of electroluminescent pigments in the totalmass of the electroluminescent layer (degree of filling) is 20 to 75 wt.%, preferably 50 to 70 wt. %.

The electroluminescent pigments used in the electroluminescent layerhave in general a thickness of 1 to 50 μm, preferably 5 to 25 μm.

Thick-film AC-EL systems have been well known since Destriau in 1947,and are applied to ITO-PET films generally by means of screen printing.Since zinc sulfide electroluminophores experience a very highdegradation in operation and specifically at elevated temperatures andin a water vapour atmosphere, nowadays in general microencapsulated ELpigments are used for long-life thick-film AC-EL lamp structures. It ishowever also possible to use non-microencapsulated pigments in the ELelement according to the invention, as is discussed further hereinafter.

EL elements are understood in the context of the present invention tomean thick-film EL systems that are operated by means of alternatingvoltage at normally 100 volts and 400 Hz and in this way emit aso-called cold light of a few cd/m² up to several 100 cd/m² or more. ELscreen printing pastes are generally used in such inorganic thick-filmalternating voltage EL elements.

Such EL screen printing pastes are generally formulated on the basis ofinorganic substances.

Suitable substances are for example highly pure ZnS, CdS,Zn_(x)Cd_(1-x)S compounds of groups II and IV of the Periodic System ofthe Elements, ZnS being particularly preferably used. The aforementionedsubstances can be doped or activated and optionally also co-activated.Copper and/or manganese for example are used for the doping. Theco-activation is carried out for example with chlorine, bromine, iodineand aluminium. The content of alkali metals and rare earth metals in theaforementioned substances is generally very low, if these are present atall. Most particularly preferably ZnS is used, which is preferably dopedor activated with copper and/or manganese and is preferably co-activatedwith chlorine, bromine, iodine and/or aluminium.

Normal EL emission colours are yellow, orange, green, green-blue,blue-green and white, the emission colours white or red being able to beobtained by mixtures of suitable EL phosphors (pigments) or by colourconversion. The colour conversion can generally be implemented in theform of a converting layer and/or by admixture of appropriate dyes andpigments in the polymeric binder of the screen printing inks or in thepolymeric matrix in which the EL pigments are incorporated.

If the electroluminescent arrangement according to the invention is usedin a distinguishing sign for vehicles, it is preferred that theelectroluminescent arrangement emits the colour white.

In a further embodiment of the present invention the screen printingmatrix used for the production of the EL layer is provided with glazing,colour-filtering or colour-converting dyes and/or pigments. The emissioncolour white or a day/night light effect can be generated in this way.In a further embodiment pigments are used in the EL layer that have anemission in the blue wavelength range from 420 to 480 nm and areprovided with a colour-converting microencapsulation. The colour whitecan be emitted in this way.

In one embodiment, as pigments in the EL layer AC-P-EL pigments are usedthat have an emission in the blue wavelength range from 420 to 480 nm.In addition the AC-P-EL screen printing matrix preferably containswavelength-converting inorganic fine particles based oneuropium(II)-activated alkaline earth orthosilicate luminous pigmentssuch as (Ba, Sr, Ca)₂SiO₄:Eu²⁺ or YAG luminous pigments such asY₃Al₅O₁₂:Ce³⁺ or Tb₃Al₅O₁₂:Ce³⁺ or Sr₂GaS₄:Eu²⁺ or SrS:Eu²⁺ or(Y,Lu,Gd,Tb)₃(Al,Sc,Ga)₅O₁₂:Ce³⁺ or (Zn, Ca,Sr)(S,Se):Eu²⁺. A whiteemission can also be achieved in this way.

Corresponding to the prior art the aforementioned EL pigments can bemicroencapsulated. Due to the inorganic microencapsulation techniquesgood half-life times can be achieved. The EL screen printing systemLuxprint® for EL from E.I. du Pont de Neinours and Companies may bementioned here by way of example. Organic microencapsulation techniquesand film-wrap laminates based on the various thermoplastic films are inprinciple also suitable, but have however proved to be expensive and donot significantly prolong the service life.

Suitable zinc sulfide microencapsulated EL luminous pigments areavailable from Osram Sylvania, Inc. Towanda under the trade namesGlacierGLO™ Standard, High Brite and Long Life, and from the DurelDivision of the Rogers Corporation under the trade names 1PHS001®High-Efficiency Green Encapsulated EL Phosphor, 1PHS002® High-EfficiencyBlue-Green Encapsulated EL Phosphor, 1PHS003® Long-Life BlueEncapsulated EL Phosphor, 1PHS004® Long-Life Orange Encapsulated ELPhosphor.

The mean particle diameters of the suitable microencapsulated pigmentsin the EL layer are in general 15 to 60 μm preferably 20 to 35 μm.

Non-microencapsulated fine grain EL pigments, preferably with a highservice life, can as already mentioned also be used in the EL layer ofthe EL element according to the invention. Suitablenon-microencapsulated fine grain zinc sulfide electroluminescentphosphors are disclosed for example in U.S. Pat. No. 6,248,261 and in WO01/34723. These preferably have a cubic crystal lattice structure. Thenon-microencapsulated pigments preferably have mean particle diametersof 1 to 30 um, particularly preferably 2 to 15 μm, most particularlypreferably 5 to 10 μm.

Specifically, non-microencapsulated EL pigments with smaller pigmentdimensions down to below 10 μm can be used.

Thus, unencapsulated pigments can be admixed with the suitable screenprinting inks according to the present invention, preferably havingregard to the special hygroscopic properties of the pigments, preferablythe ZnS pigments. In this connection in general binders are used that onthe one hand have a good adhesion to so-called ITO layers (indium-tinoxide layers) or to intrinsically conducting polymeric transparentlayers, and that on the other hand have a good insulating effect,strengthen the dielectric and thereby effect an improvement of thebreakdown strength at high electric field strengths, and in addition inthe cured state exhibit a good water vapour barrier effect andadditionally protect the EL pigment and prolong the service life.

In one embodiment of the present invention pigments that are notmicroencapsulated are used in the AC-P-EL luminous layer.

The half-life times of the suitable pigments in the electroluminescentlayer, i.e. the time during which the initial brightness of theelectroluminescent element according to the invention has fallen byhalf, are in general at 100 volts and 80 volts and 400 Hz, 400 hours upto 5,000 hours, specifically 1,000 to 3,500 hours.

The brightness values (EL emission) are in general 1 to 200 cd/m²,preferably 3 to 100 cd/m², particularly preferably 5 to 40 cd/m²; withlarge luminous surface areas the brightness values are preferably in therange from 1 to 50 cd/m².

Pigments with longer or shorter half-life times and higher or lowerbrightness values can however also be used in the EL layer of the ELelement according to the invention.

In a further embodiment of the present invention the pigments present inthe EL layer have such a small mean particle diameter, or such a lowdegree of filling in the EL layer, or the individual EL layers areconfigured geometrically so small, or the interspacing of the individuallayers is chosen so large, that the EL element in the case ofnon-electrically activated luminous structures is configured to be atleast partially transparent or to ensure transmissibility. Suitablepigment particle diameters, degrees of filling, dimensions of theluminous elements and interspacings of the luminous elements have beenmentioned hereinbefore.

The layer contains the aforementioned, optionally doped ZnS crystals,preferably microencapsulated as described above, preferably in an amountof 40 to 90 wt. %, more preferably 50 to 80 wt. %, particularlypreferably 55 to 70 wt. %, in each case referred to the weight of thepaste. One-component and preferably two-component polyurethanes can beused as binder. Preferred according to the invention are highly flexiblematerials from Bayer MaterialScience AG, for example the lacquer rawmaterials of the Desmophen and Desmodur ranges, preferably Desmophen andDesmodur, or the lacquer raw materials of the Lupranate, Lupranol,Pluracol or Lupraphen ranges from BASF AG. As solvents, ethoxypropylacetate, ethyl acetate, butyl acetate, methoxypropyl acetate, acetone,methyl ethyl ketone, methyl isobutyl ketone, cyclohexanone, toluene,xylene, solvent naphtha 100 or arbitrary mixtures of two or more ofthese solvents can be used in amounts of preferably 1 to 50 wt. %,preferably 2 to 30 wt. %, particularly preferably 5 to 15 wt. %, in eachcase referred to the total amount of paste. Furthermore other highlyflexible binders, for example those based on PMMA, PVA, in particularmowiol and poval from Kuraray Europe GmbH (now called KuraraySpecialties) or polyviol from Wacker AG, or PVB, in particular mowitalfrom Kuraray Europe GmbH (B 20H, B 30 T, B 30H, B 30 HH, B 45H, B 60 T,B 60H, B 60 HH, B 75H), or pioloform, in particular pioloform BR18, BM18or BT18, from Wacker AG, can be used. When using polymeric binders suchas for example PVB, solvents such as methanol, ethanol, propanol,isopropanol, diacetone alcohol, benzyl alcohol, 1-methoxypropanol-2,butyl glycol, methoxybutanol, dowanol, methoxypropyl acetate, methylacetate, ethyl acetate, butyl acetate, butoxyl, glycolic acid n-butylester, acetone, methyl ethyl ketone, methyl isobutyl ketone,cyclohexanone, toluene, xylene, hexane, cyclohexane, heptane as well asmixtures of two or more of the aforementioned solvents can furthermorebe added in amounts of 1 to 30 wt. % referred to the total weight of thepaste, preferably 2 to 20 wt. %, particularly preferably 3 to 10 wt. %.

In addition 0.1 to 2 wt. % of additives can be included in order toimprove the flow behaviour and the flow. Examples of flow improvers areAdditol XL480 in butoxyl in a mixing ratio of 40:60 to 60:40. As furtheradditives 0.01 to 10 wt. %, preferably 0.05 to 5 wt. %, particularlypreferably 0.1 to 2 wt. %, in each case referred to the total weight ofthe paste, of rheology additives can be included, which reduce thesettling behaviour of pigments and fillers in the paste, for example BYK410, BYK 411, BYK 430, BYK 431 or arbitrary mixtures thereof.

Particularly preferred formulations according to the invention ofprinting pastes for the production of the EL luminous pigment layer ascomponent BC contain:

Content/ Content/ Content/ Content/ Substance wt. % wt. % wt. % wt. %Pigment 55.3 69.7 64.75 65.1 (Osram Sylvania) Desmophen 18.5 11.9 12.713.1 D670 (BMS) Desmodur 16.0 9.0 12.4 11.3 N75 MPA (BMS) Ethoxypropyl9.8 9.1 9.9 10.2 acetate Additol XL480 0.4 0.3 0.25 0.3 (50 wt. % inbutoxyl) Content/ Content/ Content/ Substance wt. % wt. % wt. % Pigment61.2 65.1 69.7 (Osram Sylvania) Desmophen 15.2 12.7 11.9 D670 (BMS)Desmodur 13.1 11.4 9.0 N75 MPA (BMS) Methoxypropyl 10.2 5.5 4.9 acetateEthoxypropyl 0 5 4.2 acetate Additol XL480 0.3 0.3 0.3 (50 wt. % inbutoxyl) Content/ Content/ Substance wt. % wt. % Pigment 61.2 69.7(Osram Sylvania) Desmophen 17.7 14.1 1800 (BMS) Desmodur 9.9 7.9 L67MPA/X (BMS) Ethoxypropyl 10.8 8.0 acetate Additol XL480 0.4 0.3 (50 wt.% in butoxyl)

In a further, particularly preferred embodiment the electroluminescentlayer in the electroluminescent arrangement is based on anelectroluminescent phosphor emitting the colour green and on colourconversion pigments that are homogeneously dispersed in theelectroluminescent layer. Suitable colour conversion pigments for thispurpose are for example “EL Color Converting Pigments FA-000 Series”from the Sinloihi Co., Ltd. Japan. It is also possible to admix acolour-converting substance such as rhodamine, so that a white emissionis obtained. The electroluminescence emission in the region of thecolour white is particularly preferred if the electroluminescentarrangement is used in an identification plate for vehicles.

In addition, all commercially available EL pastes that possess thenecessary forming/shaping properties can be used to produce the ELlayer. In particular the paste systems from Dupont are suitable,especially those from the Luxprint range.

Electrodes

The EL element according to the invention comprises a first, at leastpartially transparent, front electrode BA and a second electrode, therear electrode BE.

The expression “at least partially transparent” is understood in thecontext of the present invention to denote an electrode that isconstructed of a material that has a transmission of in general morethan 60%, preferably more than 70%, particularly preferably more than80% and especially more than 90%.

The rear electrode BE need not necessarily be transparent.

Suitable electrically conducting materials for the electrodes are knownto the person skilled in the art. In principle several types ofelectrodes are available for the production of thick-film EL elementsexhibiting alternating voltage excitation. These include on the one handindium-tin oxide electrodes (indium-tin oxides, ITO) applied bysputtering or vapour deposition to plastics films. They are extremelythin (a few 100 Å) and have the advantage of a high transparencycombined with a relatively low sheet resistance (ca. 60 to 600Ω).

Furthermore printing pastes with ITO or ATO (indium-tin oxides,antimony-tin oxide) or intrinsically conducting transparent polymerpastes can be used, from which flat electrodes can be produced by meansof screen printing. At a thickness of ca. 5 to 20 μm such electrodeshave only a relatively small transparency with a high sheet resistance(up to 50 kΩ). They can be applied largely in any desired structuralshape, and indeed also on structured surfaces. In addition they have arelatively good laminability. Also, non-ITO screen printing layers(wherein the term “non-ITO” includes all screen printing layers that arenot based on indium-tin oxide (ITO)), in other words intrinsicallyconducting polymeric layers with normally nanoscale electricallyconducting pigments, for example the ATO printing pastes with thedesignations 7162E or 7164 from DuPont, the intrinsically conductingpolymer systems, such as the Orgacon® system from Agfa, the Baytron®poly-(3,4-ethylenedioxythiophene) system from H. C. Starck GmbH, theOrmecon system termed organic metal (PEDT-conductive polymerpolyethylene-dioxythiophene), conducting coating or printing pastesystems from Panipol OY and optionally with highly flexible binders, forexample based on PU (polyurethanes), PMMA (polymethyl methacrylate), PVA(polyvinyl alcohol), or modified polyaniline, can be used. Preferablythe Baytron® poly-(3,4-ethylenedioxythiophene) system from H. C. StarckGmbH is used as the material of the at least partially transparentelectrode of the electroluminescent element. Examples of electricallyconducting polymer films are polyanilines, polythiophenes,polyacetylenes, polypyrroles (Handbook of Conducting Polymers, 1986),with and without a metal oxide filling.

According to the invention, 10 to 90 wt. %, preferably 20 to 80 wt. %,particularly preferably 30 to 65 wt. %, in each case referred to thetotal weight of the printing paste, of Clevios P, Clevios PH, Clevios PAG, Clevios P HCV4, Clevios P HS, Clevios PH 500, Clevios PH 510 orarbitrary mixtures thereof, are preferably used for the formulation of aprinting paste for the production of the at least partially transparentelectrode BA. Dimethyl sulfoxide (DMSO), N,N-dimethylformamide,N,N-dimethylacetamide, ethylene glycol, glycerol, sorbitol, methanol,ethanol, isopropanol, n-propanol, acetone, methyl ethyl ketone,dimethylaminoethanol, water or mixtures of two, three or more of theaforementioned compounds can be used as solvent. The amount of solventcan vary in wide ranges in the printing paste. For example, oneformulation according to the invention of a paste can contain 55 to 60wt. % of solvent, whereas in another formulation according to theinvention about 35 to 45 wt. % of a solvent mixture of two or moresubstances can be used. Furthermore Silquest A187, Neo Rez R986, Dynol604 and/or mixtures of two or more of these substances can be includedas surfactant additive and bonding activator. The amount of thesesubstances is 0.1 to 5.0 wt. %, preferably 0.3 to 2.5 wt. %, referred tothe total weight of the printing paste.

As binder, the formulation can contain for example Bayderm Finish 85 UD,Bayhydrol PR340/1, Bayhydrol PR135 or arbitrary mixtures thereof,preferably in amounts of about 0.5 to 10 wt. %, preferably 3 to 5 wt. %.The polyurethane dispersions used according to the invention, whichafter the drying of the layer form the binder for the conducting layer,are preferably aqueous polyurethane dispersions.

According to the invention, particularly preferred formulations ofprinting pastes for the production of the partially transparentelectrode BA contain:

Content/ Content/ Content/ Content/ Substance wt. % wt. % wt. % wt. %Clevios P HS 33 48 40 42.2 (H. C. Starck) Silquest A187 0.4 0.5 1.2 1.0(OSi Specialties) N-methyl-pyrrolidone 23.7 14.4 10.3 13.3 Diethyleneglycol 26.3 20.7 30.0 25.4 Proglyde/DMM 12.6 12.4 14.5 13.6 BaydermFinish 4.0 4.0 4.0 4.5 85 UD (Lanxess) Content/ Content/ Substance wt. %wt. % Clevios P HS 33 40 (H. C. Starck) Silquest A187 0.4 1.2 (OSiSpecialties) N-methyl-pyrrolidone 23.7 10.3 Diethylene glycol 26.3 30.0Proglyde/DMM 12.6 14.5 Bayhydrol P340/1 4.0 4.0

By way of departure from the formulations mentioned above for thepartially transparent electrode BA, the following ready-for-use,commercially obtainable printing pastes mentioned here by way of examplecan also be used according to the invention as finished formulations:the Orgacon EL-P1000, EL-P3000, EL-P5000 or EL-P6000 range from Agfa,preferably the EL-P3000 and EL-P6000 range (in particular for formableuses).

These electrode materials can be applied for example by means of screenprinting, knife coating, sputtering, spraying and/or brushing oncorresponding carrier materials (substrates), which are then preferablydried at low temperatures of for example 80° to 120° C.

Moreover, tin oxide (MESA) pastes can also be used as correspondingelectrode material.

In a preferred alternative embodiment the application of theelectrically conducting coating is carried out in vacuo orpyrolytically.

Particularly preferably in the alternative embodiment the electricallyconducting coating is a metallic or metal oxide, thin and largelytransparent layer produced in vacuo or pyrolytically, which preferablyhas a sheet resistance of 5 mΩ to 3,000Ω/square, particularly preferablya sheet resistance of 0.1 to 1,000Ω/square, most particularly preferably5 to 30Ω/square, and in a further preferred embodiment has a daylighttransmissibility at least greater than 60% (>60 to 100%) and inparticular greater than 76% (>76 to 100%).

Furthermore electrically conducting glass can also be used as electrode.

A particularly preferred type of electrically conducting and highlytransparent glass, in particular float glass, are pyrolytically producedlayers that have a high surface hardness and whose electrical surfaceresistance can be adjusted in a very wide range from in general a fewmilliohms up to 3,000Ω/square.

Such pyrolytically coated glasses can be readily shaped/formed and havea good scratch resistance, and in particular scratches do not lead to anelectrical interruption of the electrically conducting surface layer,but simply to a generally slight increase of the sheet resistance.

Furthermore, pyrolytically produced conducting surface layers are due tothe heat treatment diffused to such a large extent and anchored in thesurface that in a subsequent material application an extremely highadhesive bonding with the glass substrate is produced, which is likewisevery advantageous for the present invention. In addition such coatingshave a good homogeneity, and therefore only a slight variation in thesurface resistance over large surfaces. This property is likewise anadvantage for the present invention.

Electrically conducting and highly transparent thin layers can beproduced substantially more efficiently and cost-effectively on a glasssubstrate, which is preferably used according to the invention, than onpolymeric substrates such as PET, PMMA or PC. The electrical sheetresistance in the case of glass coatings is on average more favourableby a factor of 10 than on a polymeric film of comparable transparency,thus for example 3 to 10 ohm/square in the case of glass layers comparedto 30 to 100Ω/square on PET films.

The rear electrode component BE is—as in the case of the at leastpartially transparent electrode—a flat electrode, which however need notbe transparent or at least partially transparent. This is in generalapplied to the insulating layer, if present. If no insulating layer ispresent, then the rear electrode is applied to the layer containing atleast one luminous substance that can be excited by an electrical field.In an alternative embodiment the rear electrode is applied to thesubstrate A.

The rear electrode is in general formed from electrically conductingmaterials based on inorganic or organic substances, for example frommetals such as silver, wherein preferably those materials are used thatare not damaged if the isostatic high-pressure fanning process is usedto produce the three-dimensionally formed sheet element according to theinvention. Suitable electrodes include furthermore in particularpolymeric electrically conducting coatings. In this case the coatingsalready mentioned in connection with the at least partially transparentelectrode can be used.

Moreover, those polymeric electrically conducting coatings known to theperson skilled in the art that are not at least partially transparent,can be employed.

The formulation of the printing paste for the rear electrode can in thisconnection correspond to that of the partially transparent electrode.

By way of departure from this formulation, the following formulation canhowever also be used according to the invention for the rear electrode.

30 to 90 wt. %, preferably 40 to 80 wt. %, particularly preferably 50 to70 wt. %, in each case referred to the total weight of the printingpaste, of the conducting polymers Clevios P, Clevios PH, Clevios P AG,Clevios P HCV4, Clevios P HS, Clevios PH, Clevios PH 500, Clevios PH 510or arbitrary mixtures thereof, are used for the formulation of aprinting paste for the production of the rear electrode. Dimethylsulfoxide (DMSO), N,N-dimethylformamide, N,N-dimethylacetamide, ethyleneglycol, glycerol, sorbitol, methanol, ethanol, isopropanol, n-propanol,acetone, methyl ethyl ketone, dimethylaminoethanol, water or mixtures oftwo, three or more of these solvents can be used as solvent. The amountof solvent that is used can vary in wide ranges. Thus, one formulationof a paste according to the invention can contain 55 to 60 wt. % ofsolvent, whereas in another formulation according to the invention about40 wt. % of a solvent mixture of three solvents is used. Furthermore,Silquest A187, Neo Rez R986, Dynol 604 or mixtures of two or more ofthese substances can be used as surfactant additive and bondingactivator, preferably in an amount of 0.7 to 1.2 wt. %. The formulationcan contain for example 0.5 to 1.5 wt. % of UD-85, Bayhydrol PR340/1,Bayhydrol PR135 or arbitrary mixtures thereof as binder.

In a further embodiment according to the invention the rear electrodecan be filled with graphite. This can be accomplished by adding graphiteto the formulations described above. By way of departure from theformulation mentioned above for the rear electrode, the followingready-for-use, commercially obtainable printing pastes already mentionedhere by way of example can also be used according to the invention: theOrgacon EL-P1000, EL-P3000, EL-P5000 or EL-P6000 range from Agfa,preferably the EL-P3000 and EL-P6000 range (for formable uses). Graphitecan also be added in this case.

The printing pastes of the Orgacon EL-P4000 range, in particular OrgaconEL-P4010 and EL-4020, can also be used specifically for the rearelectrode. Both can be mixed with one another in any desired ratio.Orgacon EL-P4010 and EL-4020 already contain graphite.

Graphite pastes that can also be obtained commercially, for examplegraphite pastes from Acheson, in particular Electrodag 965 SS orElectrodag 6017 SS, can be used as rear electrode.

A particularly preferred formulation according to the invention of aprinting paste for producing the rear electrode BE contains:

Content/ Content/ Content/ Substance wt.-% wt.-% wt.-% Clevios P HS 58.050.7 64.0 Silquest A187 2.0 1.0 1.6 NMP (e.g. BASF) 17.0 12.1 14.8 DEG10.0 23.5 5.9 DPG/DMM 10.0 8.6 10.2 Bayderm Finish 3.0 4.1 3.5 85 UD(Lanxess) Content/ Content/ Substance wt.-% wt.-% Clevios P HS 58.0 50.7Silquest A187 2.0 1.0 NMP (e.g. BASF) 17.0 12.1 DEG 10.0 23.5 DPG/DMM10.0 8.6 Bayhydrol P340/1 3.0 4.1

In the context of the present invention it is also possible to useintrinsically conducting polymers as electrode material. The sheetresistance of corresponding electrodes formed from intrinsicallyconducting polymers should in general be 100 to 2000Ω/square,particularly preferably 200 to 1500Ω/square, especially 200 to1000Ω/square, and specifically 300 to 600Ω/square.

The electrically conducting materials described above can in addition beapplied to a substrate formed as carrier material. Metal foils, metallayers and thermoplastic films are for example suitable as carriermaterial.

The rear electrode is—as in the case of the at least partiallytransparent cover electrode—a flat electrode, which however need not betransparent or at least partially transparent. This electrode is ingeneral constructed of inorganically or organically based electricallyconducting materials, for example metals such as silver. Suitableelectrodes are furthermore in particular polymeric electricallyconducting coatings. In this connection the coatings already mentionedabove in connection with the at least partially transparent coverelectrode can be used. In addition, those polymeric electricallyconducting coatings known to the person skilled in the art and which arenot at least partially transparent can also be used.

Suitable materials of the rear electrode are thus preferably selectedfrom the group consisting of metals such as silver, carbon, ITOsilk-screen printing layers, ATO silk-screen printing layers, non-ITOsilk-screen printing layers, in other words intrinsically conductingpolymeric systems containing normally nanoscale electrically conductingpigments, for example ATO silk-screen printing pastes with the referenceidentification 7162E or 7164 from DuPont, intrinsically conductingpolymer systems such as the Orgacon® System from Agfa, the Baytron®poly-(3,4-ethylenedioxythiophene) system from H. C. Starck GmbH, thesystem from Ormecon termed organic metal (PEDT conductive polymerpolyethylene-dioxythiophene), electrically conducting coating andprinting ink systems from Panipol Oy and optionally with highly flexiblebinders, for example based on PU (polyurethanes), PMMA (polymethylmethacrylate), PVA (polyvinyl alcohol) or modified polyaniline, whereinmetals such as silver or carbon can be added to, and/or incorporated asa layer in, these materials in order to improve their electricalconductivity.

Moreover, it is possible for the cover electrode BA to include particleswith nanostructures.

It is also possible for the rear electrode BE to include particles withnanostructures.

In a third configuration both the cover electrode BA and the rearelectrode BE contains particles with nanostructures.

In the scope of the present invention the expression “particles withnanostructures” is understood to denote nano-scale material structuresthat are selected from the group consisting of single-wall carbonnanotubes (SWCNTs), multi-wall carbon nanotubes (MWCNTs), nanohorns,nanodisks, nanocones (i.e. structures with conically shaped jackets),metallic nanowires and combinations of the aforementioned particles.Corresponding particles with nanostructures based on carbon can forexample consist of carbon nanotubes (single-wall and multi-wall), carbonnanofibres (herringbone, platelet-type, screw-type) and the like.

The production of these single-walled carbon nanotubes is known to theperson skilled in the art and reference can be made to correspondingprocesses in the prior art. These include for example catalytic chemicalgaseous phase deposition CCVD:

These processes often produce fractions that differ as regards theirdiameter, length, chirality and electronic properties. They occur in theform of bundles and are often mixed with a proportion of amorphouscarbon. The SWCNTs are separated out from these fractions.

The separation processes known hitherto for SWCNTs are based on electrontransfer effects on metallic SWCNTs treated with diazonium salts, ondielectrophoresis, on a special chemical affinity of semiconductingcarbon nanotubes for octadecylamines and on carbon nanotubes that arecovered with single-strand DNA. The selectivity of these methods can befurther improved by intensive centrifugation of pretreated dispersionsand the use of ion exchange chromatography. In the context of thepresent invention preferably fraction-pure single-walled carbonnanotubes are used, i.e. fractions of single-walled carbon nanotubesthat differ in terms of a parameter selected from the group consistingof diameter, length, chirality and electronic properties, by at most50%, particularly preferably by at most 40%, especially by at most 30%,specifically by at most 20% and most specifically by at most 10%.

With regard to metallic nanowires, reference is made to WO 2007/022226A2, the disclosure of which regarding the nanowires disclosed therein isincorporated by way of reference in the present invention. Theelectrically highly conducting and largely transparent silver nanowiresdescribed in WO 2007/022226 A2 are particularly suitable for the presentinvention.

The production of the other particles with nanostructures is known tothe person skilled in the art and is described in the correspondingdocuments of the prior art.

Conducting Tracks, Connections of the Electrodes

In the case of large area luminous elements with a luminous capacitorstructure, the surface conductivity plays a significant role as regardsa uniform luminous density. In the case of large area luminous elementsso-called busbars are frequently used as conducting tracks, i.e.component BF, especially with semiconducting LEPs (light-emittingpolymers), PLED and/or OLED systems, in which relatively large currentsflow. In this case very highly electrically conducting tracks are formedin the manner of a cross. In this way a large surface area for exampleis subdivided into four small areas. The voltage drop in the middleregion of a luminous surface is thereby significantly reduced and theuniformity of the luminous density and the decrease in brightness in thecentre of a luminous field is reduced.

In the case of a zinc sulfide particular EL field employed in oneembodiment according to the invention, in general alternating voltagesgreater than 100 volts and up to more than 200 volts are applied, andvery low currents flow if a good dielectric material or good insulationare employed. In the ZnS thick-film AC-EL element according to theinvention the problem of current loading is therefore substantially lessthan in the case of semiconducting LEP or OLED systems, so that the useof busbars is not absolutely essential, but instead large area luminouselements can already be installed without using busbars.

Preferably according to the invention it is sufficient if the silver busin the case of areas smaller than DIN A3 is printed only on the edge ofthe electrode layer BA or BE; with areas larger than DIN A3 it ispreferred according to the invention if the silver bus forms at least anadditional conducting track.

The electrical connections can be produced for example by usingelectrically conducting and stovable pastes containing tin, zinc,silver, palladium, aluminium and further suitable conducting metals, orcombinations and mixtures or alloys thereof.

In this connection the electrically conducting contacting strips aregenerally applied by means of screen printing, brush application,ink-jet, knife coating, roller application, spraying, or by means ofdispenser application or comparable application methods known to theperson skilled in the art, to the electrically conducting and at leastpartially transparent thin coatings, and are then generally heat treatedin an oven so that strips normally applied laterally along a substrateedge can be effectively contacted in an electrically conducting mannerby means of soldering, clamping or plug-in connection.

So long as only very small electrical outputs have to be initiated onelectrically conducting coatings, spring contacts or carbon-filledrubber elements or so-called zebra rubber strips are sufficient.

Pastes based on silver, palladium, copper or gold-filled polymeradhesives are preferably used as conducting adhesive pastes.Self-adhesive, electrically conducting strips of for example tin-platedcopper foil with an electrically conducting adhesive in the z-directioncan likewise be applied by contact pressing.

The adhesive layer is in this case generally uniformly pressed in byexerting a surface pressure of a few N/cm², and depending on theimplementation, values of 0.013 ohm/cm² (for example conductive copperfoil tape VE 1691 from the company D & M International, A-8451Heimschuh) or 0.005 ohm (for example type 1183 from 3M ElectricalProducts Division, Austin, Tex. USA; according to MIL-STD-200 Method 307maintained at 5 psi/3.4 N/cm² measured over 1 sq.in. surface area) or0.001 ohm (for example type 1345 from the 3M company) or 0.003 ohm (forexample type 3202 from the company Holland Shielding Systems BV) arethereby achieved.

The contacting can however be carried out by all conventional methodsknown to the person skilled in the art, for example crimping, pluggingin, clamping, riveting or bolting/screwing.

Dielectric Layer

The EL element according to the invention preferably comprises at leastone dielectric layer, component BD, which is provided between the rearelectrode, component BE, and the EL layer, component BC.

Suitable dielectric layers are known to the person skilled in the art.Suitable layers often include highly, dielectrically acting powders,such as for example barium titanate, which are preferably dispersed influorene-containing plastics or in cyano-based resins. Examples ofparticularly suitable particles are barium titanate particles in therange of preferably 1.0 to 2.0 μm. With a high degree of filling thesecan produce a relative dielectric constant of up to 100.

The dielectric layer has a thickness of generally 1 to 50 μm, preferably2 to 40 μm, particularly preferably 5 to 25 μm, especially 8 to 15 μm.

The EL element according to the invention can in one embodiment alsoadditionally contain a further dielectric layer, which layers arearranged above one another and together improve the insulation effect,or which is interrupted by a floating electrode layer. The use of asecond dielectric layer can depend on the quality and pinhole freedom ofthe first dielectric layer.

As fillers, inorganic insulating materials are used, which are known tothe person skilled in the art from the literature and include forexample: BaTiO₃, SrTiO₃, KNbO₃, PbTiO₃, LaTaO₃, LiNbO₃, GeTe, Mg₂TiO₄,Bi₂(TiO₃)₃, NiTiO₃, CaTiO₃, ZnTiO₃, Zn₂TiO₄, BaSnO₃, Bi(SnO₃)₃, CaSnO₃,PbSnO₃, MgSnO₃, SrSnO₃, ZnSnO₃, BaZrO₃, CaZrO₃, PbZrO₃, MgZrO₃, SrZrO₃,ZnZrO₃ and lead zirconate-titanate mixed crystals or mixtures of two ormore of these fillers. Preferred fillers according to the invention areBaTiO₃ or PbZrO₃ or mixtures thereof, preferably in filling amounts of 5to 80 wt. %, preferably 10 to 75 wt. %, particularly preferably 40 to 70wt. %, in each case referred to the total weight of the paste, in thepaste used to produce the insulating layer. Examples of particularlysuitable particles are barium titanate particles in the range frompreferably 1.0 to 2.0 μm. These can with a high degree of fillingproduce a relative dielectric constant of up to 100.

One-component or preferably two-component polyurethane systems can beused as binder for this layer, preferably the systems available fromBayer MaterialScience AG, particularly preferably Desmodur and Desmophenor the lacquer raw materials of the Lupranate, Lupranol, Pluracol orLupraphen range from BASF AG; from Degussa AG (Evonik), preferablyvestanate, particularly preferably vestanate T and B; or from the DowChemical Company, preferably vorastar. Furthermore highly flexiblebinders can also be used, for example those based on PMMA, PVA, inparticular mowiol and poval from Kuraray Specialties Europe GmbH orpolyviol from Wacker AG, or PVB, in particular mowital from KuraraySpecialties Europe GmbH (B 20H, B 30 T, B 30 H, B 30 HH, B 45 H, B 60 T,B 60 H, B 60 HH, B 75 H), or pioloform, in particular pioloform BR18,BM18 or BT18, from Wacker AG. In particular fluorene-containing plasticsor cyano-based resins can also be used as binder matrix.

As solvents there may for example be used ethyl acetate, butyl acetate,1-methoxypropyl acetate-2, toluene, xylene, solvesso 100, shellsol A ormixtures of two or more of these solvents. If for example PVB is used asbinder, the paste can also contain methanol, ethanol, propanol,isopropanol, diacetone alcohol, benzyl alcohol, 1-methoxypropanol-2,butyl glycol, methoxybutanol, dowanol, methoxypropyl acetate, methylacetate, ethyl acetate, butyl acetate, butoxyl, glycolic acid n-butylester, acetone, methyl ethyl ketone, methyl isobutyl ketone,cyclohexanone, toluene, xylene, hexane, cyclohexane, heptane, as well asmixtures of two or more of the aforementioned solvents, in amounts of 1to 30 wt. % referred to the total weight of the paste, preferably 2 to20 wt. %, particularly preferably 3 to 10 wt. % Furthermore additivessuch as flow improvers and rheology additives can be added in order toimprove the properties. Examples of flow improvers are Additol XL480 inbutoxyl in a mixing ratio of 40:60 to 60:40. The paste can contain asfurther additives 0.01 to 10 wt. %, preferably 0.05 to 5 wt. %,particularly preferably 0.1 to 2 wt. %, in each case referred to thetotal weight of paste. As rheology additives, which reduce the settlingbehaviour of pigments and fillers in the paste, there can for example beused BYK 410, BYK 411, BYK 430, BYK 431 or arbitrary mixtures thereof.

Particularly preferred formulations according to the invention of aprinting paste for the production of the insulating layer as componentBB and/or BD contain:

Content/ Content/ Content/ Content/ Substance wt. % wt. % wt. % wt. %BaTiO₃ 50 50 50 55 Desmophen 25 25 25 22.5 1800 (BMS) Desmodur 14 14 1411.4 L67 MPA/X (BMS) Ethoxypropyl 8.7 0 4 0 acetate Methoxypropyl 0 8.74.7 8.6 acetate Additol XL480 2.3 2.3 2.3 2.5 (50 wt. % in butoxyl)BaTiO₃ 55 56.6 59.9 59.9 Desmophen 22.5 20.3 19.9 19.9 1800 (BMS)Desmodur 11.4 12.5 11.2 11.2 L67 MPA/X (BMS) Ethoxypropyl 8.6 7.6 5.7 0acetate Methoxypropyl 0 0 0 5.7 acetate Additol XL480 in 2.5 3.0 3.3 3.3butoxyl 50% Content/ Substance wt. % BaTiO₃ 55 Desmophen 22.5 1800 (BMS)Desmodur L67 12 MPA/X (BMS) Ethoxypropyl 8 acetate Additol XL480 2.5 (50wt. % in butoxyl) BaTiO₃ 60.2 Desmophen 14.3 670 (BMS) Desmodur 12.3N75MPA (BMS) Ethoxypropyl 10.3 acetate Additol XL480 2.9 (50 wt. % inbutoxyl)

Cover Layer

In addition to the components A and B the EL element according to theinvention contains a protective layer, component CA, in order to preventa destruction of the electroluminescent element or of the possiblypresent graphical representations. Suitable materials for the protectivelayer are known to the person skilled in the art. Suitable protectivelayers CA are for example high temperature resistant protective lacquerssuch as protective lacquers containing polycarbonates and binders. Anexample of such a protective lacquer is Noriphan® HTR from Pröll,Weiβenburg.

Alternatively the protective layer can also be formulated on the basisof flexible polymers such as polyurethanes, PMMA, PVA or PVB.Polyurethanes from Bayer MaterialScience AG can be used for thispurpose. This formulation can also be provided with fillers. All fillersknown to the person skilled in the art are suitable for this purpose,for example based on inorganic metal oxides such as TiO₂, ZnO,lithopones, etc., with a degree of filling of 10 to 80 wt. % of theprinting paste, preferably a degree of filling of 20 to 70%,particularly preferably of 40 to 60%. Furthermore the formulations cancontain flow improvers as well as rheology additives. As solvents therecan be used for example ethoxypropyl acetate, ethyl acetate, butylacetate, methoxypropyl acetate, acetone, methyl ethyl ketone, methylisobutyl ketone, cyclohexanone, toluene, xylene, solvent naphtha 100 ormixtures of two or more of these solvents.

According to the invention particularly preferred formulations of theprotective lacquer CA contain for example:

Content/ Content/ Content/ Content/ Substance wt. % wt. % wt. % wt. %Desmophen 18.9 22.0 17.3 22.0 670 (BMS) Additol 1.2 0.8 1.0 0.8 XL480(50 wt. % in butoxyl) Desmodur 20.0 20.0 17.4 20.0 N75 MPA (BMS)Ethoxypropyl 4.5 8.5 4.3 0 acetate Methoxypropyl 0 0 0 8.5 acetate TiO₂55.4 48.7 60.0 48.7 Content/ Substance wt. % Desmophen 22.9 1800 (BMS)Additol XL480 1.1 (50 wt. % in butoxyl) Desmodur 12.9 L67 MPA/X (BMS)Ethoxypropyl 10.6 acetate TiO₂ 52.5

Substrates

The EL element according to the invention can comprise on one or bothsides of the respective electrodes, substrates such as for exampleglasses, plastics films or the like.

In the EL element according to the invention it is preferred if at leastthe substrate that is in contact with the transparent electrode isdesigned to be graphically glazingly translucent and opaquely coveringon the inside. An opaque covering design is understood to mean a largearea electroluminescence region that is opaquely covered by ahigh-resolution graphical design and/or is formed glazingly, for examplein the sense of red-green-blue, translucently for signalling purposes.

The electroluminescent arrangement according to the invention can beapplied via the rear electrode BE to a rear substrate, for example analuminium substrate. The electroluminescent arrangement can in thisconnection be joined to the substrate via an adhesive layer that isapplied to the rear electrode.

In a further embodiment of the present invention, in the EL arrangementaccording to the invention a layer of a protective lacquer can beprovided between the substrate and the rear electrode. If the layer of aprotective lacquer is provided in the electroluminescent arrangementaccording to the invention, then the electroluminescent arrangement canbe joined to the corresponding substrate via an adhesive layer, which inthis case is applied to the layer of the protective lacquer.

A cold-setting adhesive system as well as a hot-setting adhesive systemcan be used as adhesive system.

The adhesive system employed in the electroluminescent arrangementaccording to the invention can be formulated as a one-component systemas well as a two-component system.

The adhesive system can in one modification be based on a systemcomprising silicone, ethylene vinyl acetate, PVC or thermoplasticurethane elastomers. Of these, adhesive systems based on thermoplasticurethane elastomers are particularly preferred.

In a special embodiment an adhesive system based on thermoplasticurethane elastomers (TPU) is therefore used for the bonding of theelectroluminescent arrangement according to the invention.

The adhesive system can be formulated as a film, i.e. the adhesivesystem can be used in the form of a film. This embodiment simplifies theproduction of corresponding EL systems on account of the simplifiedhandling of the films.

As examples of materials for the adhesive layer formed as films, theremay be mentioned films known by the trade marks Dureflex®, Platilon®and/or Walopur®, which are based on thermoplastic urethane elastomers.

If corresponding film-based adhesive systems are used, then the filmscan be used together with a carrier film. In this case the thickness ofthe adhesive layer in the form of a film is 0.01 to 2 mm, particularlypreferably 0.02 to 0.5 mm, especially 0.15 to 0.40 mm.

A further substrate (cover substrate) can also be provided on the coverelectrode BA in the electroluminescent arrangement according to theinvention.

The cover substrate is likewise fixed to the electroluminescentarrangement according to the invention using the adhesive systemsmentioned above. Here too systems based on thermoplastic polyurethaneelastomers are preferred.

Since the electroluminescence generated by the arrangement according tothe invention is emitted through the cover substrate, it is preferred ifthe cover substrate is formed so as to be transparent.

In a modification of the present invention the cover substrate can bematt on the upper side, i.e. on the side facing away from theelectroluminescent arrangement.

In addition it is preferred if the substrate that is in contact with thetransparent electrode BA is a film that is cold-stretchably workablebelow the glass transition temperature Tg. In this way the possibilityis provided of working the resulting EL element three-dimensionally,preferably free of stress-whitening.

Furthermore it is preferred if the substrate that is in contact with therear electrode BE is a film that is likewise cold-stretchably workablebelow Tg. In this way the possibility is provided of working theresulting EL element three-dimensionally, preferably free ofstress-whitening.

The EL element is thus three-dimensionally workable, wherein the radiiof curvature may be less than 2 mm, preferably less than 1 mm. Theworking angle can in this connection be greater than 60°, preferablygreater than 75°, particularly preferably greater than 90° andespecially greater than 105°.

Moreover it is preferred if the EL element is three-dimensionallyworkable and in particular is cold-stretchably workable below Tg and inthis way receives a precise, worked three-dimensional shape.

The three-dimensionally worked element can be moulded on at least oneside with a thermoplastic material in an injection mould.

Production of EL Elements According to the Invention

Normally the pastes mentioned hereinbefore (screen printing pastes) areapplied to transparent plastics films or glasses, which in turn comprisea largely transparent electrically conducting coating and thereby formthe electrode for the visual display side. The dielectric material, ifpresent, and the rear side electrode are then produced by printingtechniques and/or lamination techniques.

A reverse production process is however also possible, in which first ofall the rear side electrode is produced or the rear side electrode isused in the form of a metallised film and the dielectric material isapplied to this electrode. The EL layer and following this thetransparent and electrically conducting upper electrode are thenapplied. The resultant system can then optionally be laminated with atransparent cover film and thereby protected against water vapour andalso against mechanical damage.

In one embodiment of the invention the conducting tracks (silver bus)can be applied as first layer to the substrate A. According to theinvention they are however preferably applied to the electrodes BA andBE either in two work stages, in each case individually to theelectrodes, or in one work step to the electrodes jointly.

The EL layer is normally applied by a printing technique by means ofscreen printing or dispenser application or ink-jet application, or alsoin a knife coating procedure or a roller coating method or a curtaincasting method or a transfer method, but preferably by means of screenprinting. The EL layer is preferably applied to the surface of theelectrode or to the insulating layer optionally applied to the rearelectrode. Following this, in general at least two alternating voltagesupply leads are attached at two sites arranged spaced from one anotheron at least one of the flat electrodes.

Further Configurations of the EL Arrangement According to the Invention

By using at least two EL layers it is moreover possible to produce aluminous field that differs locally and in wavelength by choosing atleast two adjacently arranged electroluminescent layers containingdifferent electroluminescent phosphor pigments.

The electroluminescent arrangement according to the invention isoperated by an electroluminescence voltage supply with an alternatingvoltage frequency in the range from 200 Hz to above 1,000 Hz. In thisconnection a coding can be created in the range of a few Hz, so that inthis way the coding can be verified by machine, for example by means ofan optoelectronic sensor or by means of a camera. Also for example thevalidity of an automobile distinguishing sign or the validity of alicense and other security-related properties can thereby be checked.

The present invention also provides for the use of an electroluminescentarrangement as described above as a decorative element and/or luminouselement in interiors or for external use, preferably on external facadesof buildings, in or on facilities and installations, in or on land,airborne or waterborne vehicles, in or on electrical or electronicdevices, or in the advertising sector.

In this connection the electroluminescent arrangement can be designed asan optically signalling element, in which the voltage levels, thevoltage differences, the frequencies and/or the frequency differencescan be controlled and modulated by the loudness level and the frequencyresponse of a music source and/or by electronic, sensory and/orcomputer-controlled regulation.

Also, the electroluminescent arrangement according to the invention canbe designed as a combined safety glass element or as an insulating glasselement.

The electroluminescent arrangement can thus be used as a visualindicator for measurable and/or sensorially detectable quantities, inparticular noise, smoke, vibration, speed, atmospheric humidity and/ortemperature.

The electroluminescent arrangement according to the invention issuitable in particular as a constituent of self-luminescent automobiledistinguishing signs. For this purpose it is however necessary that theelectroluminescent arrangement be subjected to a working step in orderto provide the automobile distinguishing sign with the correspondingautomobile distinguishing sign number. This is generally carried out bya working step executed from the rear side of the number plate so thatthe corresponding letters and numbers are pressed out forwardly from thenumber plate. This region can then be made black-opaque.

With this embossing the problem may however arise that cracks occur inthe electrode coatings, as a result of which the conductivity of theelectrode is restricted or is even interrupted in parts.

Furthermore, if there is an overloading due to the power supply this canlead to a fracture of the cover electrode and/or rear electrode of theelectroluminescent arrangement according to the invention.

The present invention solves this problem comprehensively, in that ametal grid is preferably incorporated in the respective electrodes. In aspecial embodiment of the present invention it is therefore envisagedthat at least one electrode, either the rear electrode BE or the coverelectrode BA, includes a metal grating or grid. The metal grating orgrid—in contrast to the (conventional) electrode per se—is more easilythree-dimensionally workable and, on account of the expandability of themetal grating or grid, fractures significantly less often and in generalonly under a significantly greater working, which is generally notnecessary with electroluminescent arrangements of the type underdiscussion, and also when used as a component part of a vehicledistinguishing sign.

The metal grid can in this connection be a metal grid inlay withcrossing or intersecting strands.

The metal grid can moreover in a further configuration consist ofcrossing warp strands and weft strands.

The metal grid can in general be produced using different metals. Thus,it is possible for the metal grid to consist substantially of one metal,which is selected from the group consisting of silver, copper, gold,platinum, brass, iron and nickel. It is particularly preferred if themetal grid consists substantially of silver. Depending on the electricalconductivity, the thickness of the conductor can be between 5 μm and 2mm, preferably between 10 and 200 μm. The grid can be in the form of achessboard pattern, in the form of hare wires, or of any other arbitraryshape.

In the case where the electrical conductivity of the electrode materialis interrupted—independently of the type and reason for theinterruption—the electrical conductivity of the electrodes can in thiscase continue to be maintained via the additional metal grid. Thus, evenin the event of damage the function module can be operated with avirtually unaffected performance. The fatigue properties are therebyimproved.

In a further modification of the present invention the use ofcorresponding metal grids in electroluminescent arrangements of the typeunder discussion is claimed, wherein the intended use is aimed atbridging breaks in electrical conductivity in the electrodes due toworking (deformation) of the electroluminescent arrangement.

The contacting of the electrodes of the electroluminescent arrangementaccording to the invention can take place in different ways.

Thus, in a first embodiment of the present invention it is possible forthe rear electrode and/or the cover electrode to be contacted by meansof a power supply lead. The respective power supply lead is preferablyarranged outside the electroluminescence field and is preferablyconfigured so that it can effect a uniform EL emission over the whole ELsurface. As regards this power supply lead designed as a busbar, it isconvenient to feed the alternating current flowing to the coverelectrode and rear electrode over as large an area as possible, in orderto keep the local current densities as low as possible. Otherwise thereis the danger, on account of the small thickness of the rear electrodeand cover electrode, of at least localised damage due to burning orvaporisation on account of too high a current density.

The corresponding busbars can be formed by highly conducting, printingpastes. These pastes can for example be opaque silver pastes, copperpastes or carbon pastes. Suitable printing pastes are basically notsubject to any restriction as regards the sheet resistance. Normallyhowever they have a sheet resistance in the range from below 10mΩ/square to a few 100 mΩ/square.

Especially with large surface areas and interspacings and relativelyhigh-resistive transparent electrode layers, it is suitable to usebusbars for a uniform EL emission.

In one configuration the busbar for the rear electrode BE is providedbetween the rear electrode BE and a further protective lacquer describedhereinbelow.

In one configuration the busbar for the cover electrode BA is providedbetween the cover electrode BA and the cover substrate.

The busbars can for example be joined by means of contacting strips to acorresponding electroluminescence converter (inverter).

Corresponding electrically contacting strips can in general be appliedby means of screen printing, brush application, ink-jet, knife coating,roller, by spraying or by means of dispenser application or comparableapplication methods known to the person skilled in the art, to theelectrically conducting and at least partially transparent thin coatingsand then in general heat treated in an oven so that strips normallyapplied laterally along a substrate edge can be contacted in a goodelectrically conducting manner by means of soldering, clamping,crimping, riveting, bonding or a plug-in connection.

In a special embodiment of the present invention the contacting of therear electrode and/or of the cover electrode, possibly directly via abusbar, can also take place on the rear side down to the rear substratethrough a contacting element. In this case at least two recesses for theelectrical contacts are provided in the electroluminescent arrangementvertically in the direction of the layer structure. Contacting elements,for example in the form of a screw connection, a rivet connection or asawtooth-shaped connection, are inserted in a positive locking mannerinto these recesses. The contacting elements are designed so that thereis an electrical contact through these contacting elements with thecorresponding cover electrode and rear electrode. This contact with therespective electrodes can also be effected via an already describedintermediately connected busbar, with the advantages already describedabove. This is particularly preferred since the electrical power feedthen takes place not only at the contacting element/electrode contactsite, but over a large area at the busbar/electrode contact site.

The recesses that in this embodiment are provided in theelectroluminescent arrangement according to the invention are preferablyformed in the edge region of the electroluminescent arrangement.

A mechanical fixing of the electroluminescent arrangement is alsopossible via the corresponding contact elements.

This type of contacting according to the invention and which isparticularly preferred is described in more detail in the figuresrelating to the present invention.

Independently of the precise nature of the contacting of the rear and/orcover electrode, these connections are joined to an electroluminescenceinverter (converter).

If the electroluminescent arrangement according to the invention is usedas a self-luminescent distinguishing sign on a vehicle, this powersupply can be provided by the electrical circuit of a vehicle.

In this connection it is furthermore possible for the electroluminescentarrangement to be supplied automatically with current when starting thevehicle, so that the driver of a vehicle is always assured of asufficient illumination, for example of the automobile distinguishingsigns, independently of the respective lighting conditions and withoutswitching on the electroluminescence function.

If the electroluminescent arrangement is used as a distinguishing signfor a vehicle, it is preferred if the cover substrate of the ELarrangement is formed as a plastics film. In this case it is alsoadditionally preferred if the cover substrate is a film based onpolycarbonate or a polycarbonate blend. Polycarbonate (PC) is athermally and mechanically highly stressable plastics material withoutstanding transparency. It is particularly suitable for use as a coversubstrate for the electroluminescent arrangement according to theinvention if this is used as a component part of a distinguishing signfor vehicles, since the material satisfies extremely stringent demandsas regards impact strength, scratch resistance and heat stability.

Furthermore, the cover substrate provided according to the invention inthe form of a polycarbonate film ensures that the surface of the coversubstrate has a scratch-resistant surface roughness, so that the coversubstrate does not produce any specular reflection effects. In addition,the service life of the system according to the invention is improved byvirtue of the fact that yellowing effects and embrittlement effects arelargely avoided.

In one embodiment of the present invention the polycarbonate film has onat least one side a matt surface and on the remaining side a graphicalconfiguration.

Suitable polycarbonate films are in particular polycarbonate films madefrom the materials Malcrofol®, Bayfol°, Marnot® or ProTek®. Thethickness of corresponding polycarbonate films is generally in a rangefrom 50 to 350 μm, particularly preferably 75 to 300 μm, especially 100to 250 μm.

The further structure of the electroluminescent arrangement according tothe invention, in particular when used as vehicle distinguishing signs,is not subject to any special restriction. For example, it is possibleto apply a layer of a white lacquer on the cover substrate. A reflectinglayer for example can then be provided on the layer of white lacquer. Ifa white lacquer is used in the electroluminescent arrangement accordingto the invention, then the reflecting layer can be joined to the layerof white lacquer via an adhesive. As regards this adhesive system,reference is made to the above implementations.

In order that the electroluminescent arrangement according to theinvention can be used for example as a distinguishing sign for avehicle, it is preferred if the reflecting layer, if this is used in thecontext of the electroluminescent arrangement according to theinvention, is designed to be substantially transparent.

For the present invention it has moreover proved advantageous if thereflection is increased by using hollow glass spheres. In a furtherspecial embodiment of the present invention the electroluminescentarrangement therefore comprises hollow glass spheres.

In order to improve the reflecting properties the hollow glass spherescan be added to the cover substrate.

In addition it is also possible to add hollow glass spheres to thereflecting layer, if this is used in the context of theelectroluminescent arrangement according to the invention.

Furthermore it is possible to add hollow glass spheres both to the coversubstrate and to the reflecting layer.

If in one of these modifications hollow glass spheres are used in theelectroluminescent arrangement according to the invention, then thesepreferably have a mean diameter of 5 to 200 μm, particularly preferably10 to 100 μm, especially 15 to 50 μm. The specific weight ofcorresponding hollow glass spheres is preferably 0.05 to 10 g/cm³,particularly preferably 0.1 to 5 g/cm³, especially 0.15 to 1 g/cm³.Corresponding hollow glass spheres are based for example onwater-insoluble, chemically stable soda lime borosilicate glass and arecommercially obtainable under the names Scotchlite® Glass Bubbles S60 orS60HS.

These corresponding hollow glass spheres can be applied for example in abinder matrix of the cover substrate or of the reflecting layer.

The electroluminescent arrangement described above is preferably used inautomobile distinguishing signs.

It is therefore preferred to use as rear substrate a metal substrate,preferably an aluminium substrate. In particular this can be aluminiumsheet material.

In order that the distinguishing sign for vehicles can be embossed, theelectroluminescent arrangement according to the invention is in itstotality preferably designed so that it is cold-workable and thereforefree of stress-whitening. The distinguishing sign can in particular beworked three-dimensionally, in which connection the radii of curvaturemay be less than 2 mm, preferably less than 1 mm. The working angle canin this connection be greater than 60°, preferably greater than 75°,particularly preferably greater than 90°, and in particular greater than105°.

In particular the electroluminescent arrangement according to theinvention is used as a front diaphragm blank for a number plate of avehicle. The provision of the electroluminescent arrangement as a frontdiaphragm blank is in this connection preferably effected from anarc-shaped format by means of punching tools, cutting tools and/or alaser jet system.

On the front diaphragm blank an embossing is applied from behind to thedistinguishing sign of the vehicle. The elevations formed by theembossing on the front side are then generally coloured opaque as blackregions.

Corresponding blanks generally have a layer thickness of 50 to 350 μm,particularly preferably 75 to 300 μm, especially 100 to 250 μm.

The electroluminescent arrangement according to the invention, which isused in distinguishing signs of vehicle number plates, is in generalconfigured so that in addition to the white light generated byelectroluminescence, it additionally emits colours of specificwavelengths. In this way an additional graphical configuration canoptionally be achieved. The additional wavelength-specific emission canfor example produce a symbol in the manner of a watermark on thearrangement, in which connection the watermark can also be arrangedconcealed in a time-resolved manner in order to make the distinguishingsign secure against counterfeiting.

The electroluminescent arrangements according to the invention can beproduced on conventional flat-bed and/or cylinder screen printingmachines using the multiple letter press sheet format, and during theproduction can also be provided for example with further securityfeatures by printing techniques.

The present invention accordingly also provides distinguishing signs, inparticular for vehicles, comprising the electroluminescent arrangementdescribed above, wherein the distinguishing sign is fixed in a frame andthe at least two electrical connections of the EL element are joined toan EL inverter (converter), which in general is in turn connected to theelectrical circuit of the vehicle, and is preferably automaticallysupplied with current when starting up the vehicle, and in this waycauses the EL film to luminesce.

Some examples of implementation of the invention are described in moredetail hereinafter with the aid of the drawings. These embodimentsrepresent exemplary forms of the present invention, although the presentinvention is not restricted to these embodiments.

REFERENCE NUMERALS

-   1: self-luminescent distinguishing sign-   2: perforation (recess)-   3: perforation (recess)-   4: rear substrate of aluminium-   5: adhesive layer based on TPU-   6: electroluminescent arrangement-   7: cover substrate-   8: direction of electroluminescence-   9: adhesive layer based on TPU-   10: polymeric binder matrix-   11: hollow glass spheres-   12: front-side elevations-   13: bright surface, front side-   14: frame-   15: reflecting layer in the form of a film-   16: electrical contacting elements-   17: cover electrode-   18: busbar of the cover electrode-   19: rear electrode-   20: busbar of the rear electrode-   21: electroluminescence inverter-   22: compression sleeve-   23: dielectric layer/insulating layer-   24: electroluminescent layer-   25: contact surface-   26: recess-   27: contact surface-   28: recess-   29: sealing O-ring/flat sealing ring-   30: security embossing-   31: fixing device-   32: rubber seal-   33: rubber seal-   34: contact surface-   35: contact surface-   36: conducting wire-   37: insulation-   38: unilluminated edge-   39: EL field

In FIG. 1 a self-luminescent automobile distinguishing sign 1 with thealphanumeric identification “BMS-123” is shown by way of example in planview. The electrical contacting is effected via two perforations (holes)identified by the reference numerals 2 and 3, whereby by means of theseholes 2 and 3 a mechanical fastening of the automobile distinguishingsign to the vehicle can also be effected.

FIG. 2 shows the three-dimensional layer structure of anelectroluminescent arrangement according to the invention. The base ofthe electroluminescent arrangement illustrated in this figure is ametallic, workable rear substrate 4 made of aluminium. An adhesive layer5 based on TPU is arranged on this rear substrate 4. Anelectroluminescent arrangement 6 according to the invention is providedas the next layer on this adhesive layer 5. The laminating of theelectroluminescent arrangement 6 according to the invention on the rearsubstrate 4 via the adhesive layer 5 is carried out by matchingcorresponding pressure and temperature regions. A cover substrate 7 isapplied to the electroluminescent arrangement 6 according to theinvention. The cover substrate consists of a polycarbonate film of thematerials Makrofol® or Bayfol®. The three-dimensional layer structure isillustrated graphically. The perforations 2 and 3 for the electricalcontacting are shown only diagrammatically.

In FIG. 3 the section A/B (according to FIG. 1) through theself-luminescent automobile distinguishing sign 1 is shown. Theelectroluminescence direction 8 as well as the section C is illustrated,which is described in more detail in the following FIG. 4.

In FIG. 4 the section C shown in FIG. 3 is illustrated in more detail.The base of the electroluminescent arrangement illustrated in thisfigure is again a metallic, workable rear substrate 4 made of aluminium,on which is provided an adhesive layer 5 of TPU. An electroluminescentarrangement 6 according to the invention is provided as the next layeron this adhesive layer 5. By means of a further adhesive layer 9 of TPUthe electroluminescent arrangement 6 is provided with a polymeric bindermatrix 10 containing hollow glass spheres 11. TPU is likewise used asbinder in this layer. A cover substrate 7 of a polycarbonate film with alayer thickness of 100 to 250 μm is then laminated on to the structure.The self-luminescent automobile distinguishing sign 1 is workedthree-dimensionally, whereby elevations 12 are formed on the front side,which are kept opaque in black. The region of the self-luminescentautomobile distinguishing sign 1 that does not include any elevations 12has a bright surface 13. The three-dimensional layer structure isillustrated graphically.

A contacting variant for the automobile distinguishing sign according tothe invention is illustrated in FIG. 5. The automobile distinguishingsign is in this case provided with a frame 14. The structure of theelectroluminescent arrangement according to the invention is the same asthe structure already described in the previous figures, consisting ofan aluminium substrate 4 to which is applied a first adhesive layer 5 ofTPU. An electroluminescent arrangement 6 is applied to the adhesivelayer 5 of TPU, the cover substrate 7 consisting of a polycarbonate filmbeing applied in turn to the arrangement 6. A further adhesive layer 9of TPU and a reflecting layer in the form of a film 15 are applied tothe cover substrate. The self-luminescent automobile distinguishing sign1 is worked three-dimensionally, whereby elevations 12 are formed on thefront side, which are kept opaque in black. The electrical contacting iseffected via electrical contacting elements 16, provided in the edgeregion of the automobile distinguishing sign. The electrical contactingelement 16 a is connected in an electrically conducting manner to thecover electrode 17. The electrical contact between the contactingelement 16 a and the cover electrode 17 is effected via a busbar 20,which is formed by carbon and a silver paste. The electrical contactingelement 16 b is connected in an electrically conducting manner to therear electrode 19. The electrical contact between the contacting element16 b and the rear electrode 19 is effected via a busbar 18, which isformed by carbon and a silver paste. The contact elements are connectedin an electrically conducting manner to an electroluminescence inverter21. The respective contact elements are fixed in position by compressionsleeves 22, which are provided on the rear side of the automobiledistinguishing sign 1. FIG. 5 shows two sections A and B, which aredescribed in more detail in the following figures. In FIG. 5 the coverelectrode 17 and the rear electrode 19 are not shown, but are acomponent part of the illustrated EL element 6.

The section A illustrated in FIG. 5 is described in FIG. 6. The sectionA shows the contacting of the cover electrode 17. The structure of theelectroluminescent arrangement according to the invention is the same asthat already described in the previous figures, consisting of analuminium substrate 4, to which is applied a first adhesive layer 5 ofTPU. An electroluminescent arrangement 6 according to the invention isapplied to the adhesive layer 5 of TPU, wherein the arrangement 6consists of the rear electrode 19, a dielectric layer 23, anelectroluminescent layer 24 and a cover electrode 17. The coversubstrate 7 consisting of a polycarbonate film is in turn applied to thecover electrode 17. A further adhesive layer 9 based on TPU and areflecting layer in the form of a film 15 are applied to the coversubstrate 7. The contacting of the cover electrode is effected via thecontact surface identified by the reference numeral 25. The contactingelement 16 a is not shown in FIG. 6, but has a shape so that it can beinserted in a positive locking manner into the recess 26 and contactsthe contact surface 25 of the cover electrode 17 in an electricallyconducting manner. The recess 26 can be identical to a hole 2 or 3.

The section B illustrated in FIG. 5 is described in FIG. 7. The sectionB shows the contacting of the rear electrode 19. The structure of theelectroluminescent arrangement according to the invention is the same asthat already described in the previous figures, and consists of analuminium substrate 4, to which is applied a first adhesive layer 5 ofTPU. An electroluminescent arrangement 6 according to the invention isapplied to the adhesive layer 5 of TPU, wherein the arrangement 6consists of the rear electrode 19, a dielectric layer 23, anelectroluminescent layer 24 and a cover electrode 17. The coversubstrate 7 consisting of a polycarbonate film is in turn applied to thecover electrode 17. A further adhesive layer 9 based on TPU and areflecting layer in the form of a film 15 are applied to the coversubstrate 7. The contacting is effected via the contact surfaceidentified by the reference numeral 27. The contacting element 16 b isnot illustrated in FIG. 6, but has a shape so that it can be inserted ina positive locking manner into the recess 28 and contacts the contactsurface 27 of the rear electrode 19 in an electrically conductingmanner. The contacting of the electrodes can be effected by means of abusbar.

In FIG. 8 the section B illustrated in FIG. 5 is shown in anotherconfiguration. In this configuration shown in FIG. 8 the electricalcontacting of the rear electrode serves at the same time as a mechanicalfixing. The section B shows the contacting of the rear electrode 19. Thestructure of the electroluminescent arrangement according to theinvention is the same as that already described in the precedingfigures, comprising an aluminium substrate 4, to which is applied afirst adhesive layer 5 of TPU. An electroluminescent arrangement 6according to the invention is applied to the adhesive layer 5 based onTPU, the said arrangement 6 consisting of the rear electrode 19, adielectric layer 23, an electroluminescent layer 24 and a coverelectrode 17. The cover substrate 7 consisting of a polycarbonate filmis in turn applied to the cover electrode 17. A further adhesive layer 9based on TPU and a reflecting layer in the form of a film 15 are appliedto the cover substrate 7. The automobile distinguishing sign 1 isarranged in a frame 14. A fastening to the front side of the automobiledistinguishing sign 1 is effected with the aid of a sealing O-ring 29 ora flat sealing ring, which is arranged underneath the contacting element16 b. A security embossing 30 is provided on the contacting element 16b, by means of which the code can be verified and in this way forexample the validity of the automobile distinguishing sign and thevalidity of the licence and similar security-relevant items can bechecked. The automobile distinguishing sign 1 according to the inventionis fixed mechanically to the rear side via the contacting element 16 bby means of a fastening device 31 in the form of a saw-toothed catch, arivet or a thread. Further rubber seals 32 and 33 are provided on thecontacting element 16 b.

Contact surfaces 34 and 35 are provided on the contacting element 16 b,which are in positive locking contact with the busbar 20 of the rearelectrode 19. The current required to operate the electroluminescentarrangement is supplied from an electroluminescence inverter 21 (notshown) via a conducting wire 36 that is insulated by the insulation 37.

In FIG. 9 a self-luminescent automobile distinguishing sign 1 with thealphanumeric identification “BMS-123” is shown by way of example in planview. In this embodiment two perforations (holes) 2 and 3 are providedfor the electrical contacting and the mechanical fastening. The twoperforations 2 and 3 can in principle be arranged in virtually anyposition and are preferably provided on the left-hand and right-handedges, since in this case an optimal mechanical fastening is alsopossible and the two electrically conducting flat electrodes 17 and 19(not shown) can be arranged very conveniently. In this implementationthe contacting of the cover electrode 17 occurs in the left-hand holeregion and the contacting of the rear electrode 19 occurs in theright-hand hole region. The EL field, shown hatched, extends over almostthe whole area, though normally a small edge region remains dark and theregion around the two holes is likewise implemented without an ELluminescent field.

In FIG. 10 the self-luminescent distinguishing sign 1 is showndiagrammatically in plan view, wherein simply the cover electrode 17with the busbar 18 are illustrated. The cover electrode 17 is preferablyproduced by a screen-printing technique and can thereby be arranged witha high degree of precision. The cover electrode 17 is normally arrangeddirectly adjacent to the graphical printing, including a thin whitetranslucent printing, on a transparent film as cover substrate 7 (notshown), and preferably a small edge region of about 0.5 mm to about 3.0mm is left free. Similarly, the region surrounding the right hand holeis left free for the implementation of the rear electrode contacting.The cover electrode 17 should be as transparent and as electricallyhighly conducting as possible, and is preferably designed so that thiscan be implemented by a largely cold working for the embossing of thedistinguishing sign without any crack formation. A busbar 18 is alsoshown in this FIG. 10, which is arranged in the usual configuration of abusbar with an edge region a few millimetres wide, and in addition inthe left-hand hole region covers the contacting region for the coverelectrode 17.

In FIG. 11 the self-luminescent distinguishing sign 1 is illustrateddiagrammatically in plan view, and in this connection simply the rearelectrode 19 with the grid-like busbar is shown. For reasons of cost andfunctionality a carbon paste with a sheet resistance of typically 5 to100 Ω/square is preferably used as rear electrode 19. The sheetconductivity of the carbon paste is provided by a silver paste (silverfleece) arranged in the manner of a grid, with a sheet resistance oftypically less than 100 mΩ/square down to less than 20 mΩ/square, andthe silver paste is arranged in the right-hand hole region, and here isintended to improve the contacting of the rear electrode 19. Inprinciple the silver paste can in addition also be arranged along theedges in the manner of the normal arrangement of a busbar. Since in thepresent case the rear electrode 19 does not have to be made transparent,the grid-like arrangement can be chosen and provides an additionalsecurity in the embossing procedure of the distinguishing sign, sincenormal silver pastes can be cold-worked relatively well and thepotentially high resistivity of the carbon paste is avoided. The coldworkability of the carbon paste without crack formation and thus withoutany increase in the specific sheet resistance can in addition beimproved by admixing a few tenths of a percent up to a few percent ofMWCNTs (multi-walled carbon nanotubes). Conventional MWCNTs already havea length of a few μm and in this way improve the percolation incombination with the conventional graphite particles. The admixture ofMWCNTs in the silver paste is likewise helpful and in this connectionalso improves the workability, without the danger of crack formationleading to a high resistivity. It is important to emphasise that, with asuitable arrangement of the various layers of the EL capacitor, thesilver paste impression for the grid-like rear electrode reinforcementcan at the same time serve as a busbar for the cover electrode 17 (notshown), and only this one silver paste impression reinforces theelectrical conductivity in the region of the two contacting holes 2 and3. The grid-like silver paste impression can in this connection havevirtually any arbitrary graphical configuration and can be executed witha finer grid pattern specifically in the area of the embossing for thedistinguishing sign, and need not in particular be formed as a uniformgrid, but can be designed having a progressive cross-section. Theelectrical contacting of the cover electrode 17 (not shown) and of therear electrode 19 can be effected by means of identical contactingelements. Since the EL element is operated with alternating voltage thepolarity does not have to be taken into account. With both contactings arelatively strong surface pressure can be exerted on the silver paste,since the transparent electrically conducting layer is arrangedunderneath the silver paste in the case of the front electrode, and thecarbon paste layer is arranged underneath in the case of the rearelectrode. The electrical contacting can therefore be implemented withfine, sharp-edged electrically conducting elements in the manner of amicro-piercing or nano-piercing, as well as in the manner of a crimping.

1.-29. (canceled)
 30. An electroluminescent arrangement, wherein thearrangement comprises the following structure of functional layers: (a)rear electrode as component BE; (b) dielectric layer as component BD;(c) electroluminescent layer as component BC; and (d) cover electrode ascomponent BA.
 31. The electroluminescent arrangement according to claim30, wherein the electroluminescent arrangement is applied via the rearelectrode to a rear substrate.
 32. The electroluminescent arrangementaccording to claim 31, wherein the electroluminescent arrangement isconnected to the rear substrate via an adhesive layer, which is providedbetween the rear electrode and the rear substrate.
 33. Theelectroluminescent arrangement according to claim 30, wherein a furthercover substrate is provided on the cover electrode.
 34. Theelectroluminescent arrangement according to claim 33, wherein theelectroluminescent arrangement is connected to the cover substrate viaan adhesive layer, which is provided between the cover electrode and thecover substrate.
 35. The electroluminescent arrangement according toclaim 32, wherein the adhesive system is based on a system comprisingsilicone, ethylene vinyl acetate, PVC or on a thermoplastic urethaneelastomer.
 36. The electroluminescent arrangement according to claim 35,wherein the adhesive system is formed as a film.
 37. Theelectroluminescent arrangement according to claim 30, wherein a layer ofa white lacquer is applied to the cover substrate.
 38. Theelectroluminescent arrangement according to claim 37, wherein areflecting layer is provided on the layer of the white lacquer.
 39. Theelectroluminescent arrangement according to claim 38, wherein thereflecting layer and/or the cover substrate comprises hollow glassspheres.
 40. The electroluminescent arrangement according to claim 39,wherein the hollow glass spheres have a mean diameter of 10 to 200 μm.41. The electroluminescent arrangement according to claim 30, whereinthe composition of the cover electrode and/or the composition of therear electrode includes multi-walled and/or single-walled carbonnanotubes.
 42. The electroluminescent arrangement according to claim 30,wherein the rear electrode and/or the cover electrode are contacted bymeans of a busbar.
 43. The electroluminescent arrangement according toclaim 42, wherein the rear electrode is contacted via a busbar, whereinthe busbar is provided between the rear electrode and the protectivelacquer and/or the rear substrate.
 44. The electroluminescentarrangement according to claim 42, wherein the cover electrode iscontacted via a busbar, wherein the busbar is provided between the coverelectrode and the cover substrate.
 45. The electroluminescentarrangement according to claim 30, wherein the electrical connections ofthe at least two electrodes are provided on the rear side on the rearsubstrate.
 46. The electroluminescent arrangement according to claim 45,wherein the electrical connections of the at least two electrodes areimplemented in the edge region of the electroluminescent arrangement.47. The electroluminescent arrangement according to claim 45, whereinthe at least two electrical contacts of the electroluminescentarrangement are effected by means of recesses and contacting elements,which are formed as a screw connection, rivet connection orsawtooth-shaped connection and are inserted in a positive locking mannerinto the recess, so that they effect an electrical contact with thecorresponding electrode.
 48. The electroluminescent arrangementaccording to claim 30, wherein at least one of the rear electrode or thecover electrode comprises a metal grid or grating.
 49. Theelectroluminescent arrangement according to claim 48, wherein the metalgrid consists substantially of a metal, which is selected from the groupconsisting of silver, copper, gold, platinum, brass, iron and nickel.50. The electroluminescent arrangement according to claim 49, whereinthe metal grid consists substantially of silver.
 51. Theelectroluminescent arrangement according to claim 30, wherein theelectroluminescent arrangement is used in the frame of an automobiledistinguishing sign.
 52. A distinguishing sign for an automobile whichcomprises the electroluminescent arrangement according to claim
 30. 53.A front diaphragm blank comprising the electroluminescent arrangementaccording to claim
 30. 54. A process for producing a front diaphragmblank, which comprises preparing an arcuate format from theelectroluminescent arrangement according to claim 30 and the blank isthen cut out, stamped out or otherwise fashioned, in a predeterminedsize from this arcuate format.
 55. The process according to claim 54,wherein a multiple impression arcuate format is used in the process. 56.The process according to claim 54, wherein the blank is provided withfurther security features by means of printing techniques.
 57. Adistinguishing sign comprising the electroluminescent arrangementaccording to claim 30, wherein the distinguishing sign is fixed in aframe and the at least two electrical connections are joined to an ELinverter, which optionally in turn is connected to the electricalcircuit of the vehicle and optionally is automatically supplied withcurrent when starting the vehicle, and in this way causes the EL film toluminesce.
 58. The electroluminescent arrangement according to claim 30,wherein the metal grid avoids breaks in electrical conductivity of theelectrodes of electroluminescent arrangement.